Method for the manufacture of metal carbonyls



J. V. FILL 1 'March 5, 1946.

METHOD FOR THE MANUFACTURE OF METAL CARBQNYLS INVENTOR Jaw X544 Filed May 22, 1941 (Q M ATTORNEY Patented Mar. s, 1945 METIIOD FOR THE MANUFACTURE OF.

CARBONYLS V Fill, 'Dobbs Ferry, N. guire Industries, Incorporated, New York, N. Y., a corporation of Delaware Application May 22, 1941 Serial No. 394,665

3 Claims- (Cl- 23-203).

John V. Me.

This invention relates to method and appara-- tus for the manufacture of metal carbonyls and is or special value in the making or ierro-pent'acarbonyl' (Fe(C)s) for use in making finely divided iron for magnetic cores. g

An important object of the invention is-to provide a continuous method for making metal carbonyls. In accordance with the invention, carbon monoxide gas and finely divided sponge metal are continuously fed to a reaction chamber at controlled rates while gaseous .ierro-pentacarbonyl and any excess oimetal.v are continuously withdrawn from the chamber. The metal carbonyl gas is condensed to a liquid as it is withdrawn from the chamber and this liquid is separated from any excess metal so as to provide a continuous supply of the liquid carbonyl.

Another object or the invention is to provide for a very complete and rapid reaction between metal and carbon monoxwith the-invention, finely finely divided sponge ide gas. In accordance divided sponge metal is introduced into the reaction chamber in a jet or carbon monoxide gas and the rapid stream of gas containing the metal is impinged upon another stream of carbon mon-, oxide gas moving rapidly in another direction. This exposes all surfaces of the metal particles to the gas and results in a very rapid reaction.

In order that this and other features of my inventionmay clearly be understood, I will demonoxide gas not shown,

scribe in detail a specific method embodying my invention carried out by means of the apparatus embodying my invention which is illustrated in the accompanying drawing in which: I

Fig. 1 is a diagrammatic sectional elevation of the complete apparatus;

Fig. 2 is a horizontal section on the line 2--2 of Fig. 1 showing the direction in which the injection nozzles are pointed: and

Fig. 3 is a fragmentary horizontal section of part or the wall of the reaction chamber showing a different nozzle arrangement.

In the form illustrated in Figs. 1' and 2, two nozzles II, II project into a reaction chamber Ill. The nozzles are provided with needle valves l3, It to regulate the flow through them.

Carbon monoxide gas under high pressure is red to each nozzle. I find it most desirable to have this gas under pressure of from 600 to 700 pounds per square inch, although it is .possible to operate the apparatus with any pressure between 200 and 1,000 ounds per square inch. The compressed gas for the nozzle II is introduced through a pipe I! connected to the nozzle ll by a pipe It, while the compressed gas tor the nozzle may be provided beyond the injector any large particles of the iron which are not and collects as liquid in source. In order that carbon monoxide gas depressure-regulating valve Y., assignor to I2 is introduced through the nozzle by a pipe are connected with sources The-pipes I1 and it or compressed carbon as the source from which the gas is derived is not material to this invention. 'In practice, I find it convenient to introduce into one of the supply pipes, for example, pipe 11, carbon monoxide gas derived from the decomposition of metal carbonyl carried out as shown in my co-pen'ding application Serial No. 394,656, filed May 22, 1941, and to supply the pipe IS with carbon monoxide gas from a different different sources'may be projected i and 12 at the same velocity, a I9 is provided in the pipe l1 and a pressure equalizing pipe 20 connects the two nozzles.

*Fihely divided'sponge iron pulverized to 300 mesh and free from oxide is led into the reaction chamber in the jet produced by the nozzle ll. Any powder entraining apparatus such as is used in injecting powdered coal into a furnace by means oi an air jet may be used to entrain powdered .sponge llOIlI into the stream oi compressed carbon monoxide gas entering the nozzle In the form illustrated in the drawing, the powdered sponge iron is contained in'a divided hopper 2! connected with an injector 22 introduced between the pipe l5 and the pipe it. The hopper 2| is provided with two gates 23 one oi which is closed so that one-hall! oi the hopper may be refilled with powdered sponge iron while powdered sponge iron is being drawn into the injector 22 from the other half of the hopper. This permits refilling the hopper without interrupting the operation. A- sump'2l and a collector 25 22 to collect rived from two by the nozzles l entrained by the gas jet in the injector.

The 'jets of gas from the injectors ll and i2 produce rapidly moving streams 0! gas directed in opposite directions. The two streams impact upon each other as extremely effective contact between all the surin a rapid reaction between them which produces term-carbonyl gas.

The lower portion 28 of the reaction chamber I0 is tunnel-shaped and the bottom of the chamber is connected to a vertical outlet pipe 21 which leads into a cooling chamber 28 provided with a cooling coil 29. The term-carbonyl gas is condensed to liquid term-carbonyl in this chamber the bottom of the chama pip l'l connected to shown in Fig. 2. This causes ber whence it runs through a pipe 30 into a sepaescapee a vortex in the bulge. as shown in Fig. 3. As a rator as from which it is continuously withdrawn through a pipe 36. Any excess powdered iron which may be mixed with the liquid terrocarbonyl condensed in the cooling chamber 2! is I carried with it into the separator as where it settles out from the liquid and falls into a collector 37. Any unreacted carbon monoxide gas which may pass into the separator flows upwardly around ,baflies 38 and flows out through a pipe 39.

In the operation of the apparatus which has been described, the rates at which the carbon monoxide gas and the iron enter the reaction chamber are controlled by the needle valves is, is and one of the gates 23 in such manner that the proportion between the amount oi. iron and the amount of carbon monoxide gas introduced is result, a high. velocity stream or carbon monoxide gas and entrained iron particles issuing from the injection pipe 44 impinges upon a stream direcied across the first stream by the deflector. This, like the impact between the streams from the two nozzlesoi Fig. 2. produces a rapid reacslightly in excess of that required to form ierropentacarbonyl (Fe(CO)s), namely, 3.46 pounds of iron for each 8.5 pounds of carbon monoxide. The slight excess of iron is desirable in order to avoid any danger of forming ferro-noncarbonyl (Fe(CO)a).

The apparatus described is provided with means for accurately controlling the temperature of thereaction chamber. For this purpose, the reaction chamber is provided with heat insulation 40 with a temperature-indicating thermocouple M. The pipes 16 and i8 leading to the nozzles II and I2 are provided with heating coils 42 and with thermocouples 63 to indicate the temperature at which gas is introduced into the nozzles.

While the reaction will take place at room temperature, best results are obtained when the temperature in the reaction chamber is maintained at about 200 F. Higher temperatures, such as 400 F., may be used but do not advantage.

In the modification shown in Fig. 3, an injection pipe at is directed into a cylindrical bulge 45 in the wall of the reaction chamber. The inner wall of this bulge forms a deflector which creates give any further 7 tion between the iron particles and the gas.

What I claim is: l. A method 0! making metal carbonyl, which comprises directing two high velocity jets of carbon monoxide gas into a reaction chamber, introducing powdered metal into at least one oi the jets, and imping ns'the two jets directl upon each other so asto break up the powdered metal and bring the gas into intimate contact with the metal causing a rapid reaction between them roducing metal carbonyl gas.

2. A continuous method oi making term-pentacarbonyl, which comprises continuously directing two high velocity jets of carbon monoxide gas into a reaction chamber, continuously introducing powdered metal into at least one of the jets and impinging the two Jets directly upon each other so as to break up the powdered metal and bring the gas into intimate contact with the metal causing a rapid reaction between them producing gaseous iron carbonyl, continuously withdrawing from the reaction chamber the gaseous carbonyl and any excess iron and carbon monoxide gas, condensing the gaseous carbonyl into liquid carbonyl, and separating the liquid carbonyl from any excess iron and any unreacted carbon monoxide gas, the rates at which the powdered iron and carbon monoxide are introduced being regulated to provide a slight excess of iron in order to avoid producing i'erro-nona'carbonyl.

3. The method claimed in claim 2 in which the reaction chamber is maintained at a temperature of approximately 200 F.

JOHN V. FILL. 

